US7481914B2 - Photoelectrolysis cells, and related devices and processes - Google Patents
Photoelectrolysis cells, and related devices and processes Download PDFInfo
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- US7481914B2 US7481914B2 US11/394,881 US39488106A US7481914B2 US 7481914 B2 US7481914 B2 US 7481914B2 US 39488106 A US39488106 A US 39488106A US 7481914 B2 US7481914 B2 US 7481914B2
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- photoelectrode
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- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B1/00—Electrolytic production of inorganic compounds or non-metals
- C25B1/50—Processes
- C25B1/55—Photoelectrolysis
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/36—Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
Definitions
- This invention relates generally to the production of hydrogen and oxygen by the electrolysis of water.
- the invention is directed to the production of hydrogen by the photoelectrolysis of water, using solar radiation.
- Photoelectrolytic devices are in many ways similar to photovoltaic devices, which include a p-n junction.
- the p-n junction is usually replaced by a p-electrolyte-n junction (or metal-electrolyte-n junction).
- Electron-hole pairs are generated by the absorption of light in the semiconductor electrodes.
- the semiconductor electrodes can be thought of as “photocatalysts”).
- the electron-hole pairs are separated within the photocatalyst, and are injected at the respective electrodes to produce electrochemical oxidation and reduction reactions.
- holes combine with water molecules (H 2 O) to produce an anodic oxidation reaction.
- the reverse reaction occurs at a p-type (or metal electrode), where electrons combine with protons (H+), to produce a cathodic reduction reaction.
- the net effect is a flow of electrons from the anode to the cathode, resulting in reduction at the latter (hydrogen formation), and oxidation at the former (oxygen formation).
- photoelectrolysis has the potential to provide an inexpensive source of hydrogen, while also providing a way to efficiently store energy obtained from solar energy conversion.
- photoelectrolytic processes continue to have serious drawbacks.
- the processes can be relatively slow and inefficient.
- the poor efficiency is due in large part to the bandgap characteristic of the photocatalyst(s) employed in the photoelectrolytic cells.
- Bandgap energy can be defined as the difference between the reduction potential and the oxygen potential of the cell).
- the “bandgap” is considered to be the amount of energy required to promote an electron, within its orbital configuration, from the valence band to the conduction band.
- Tandem photoelectrolytic cells which usually include two or more photocatalysts, have been used in an attempt to overcome the problems of having a single, inefficient photocatalyst.
- Various types of tandem cells have been designed.
- U.S. Pat. No. 6,936,143 (Graetzel) describes a photoelectrochemical system in which one photocell is mounted behind another cell. The design of the cells involves a color-based division for absorption of the emission spectrum. One cell which absorbs blue and green portions of the spectrum generates oxygen. The second cell includes a dye-sensitized mesoporous photovoltaic film. This cell converts yellow and red light from the spectrum, reducing protons in the first cell to hydrogen.
- tandem cells may sometimes provide greater photoelectrolytic efficiency, there are drawbacks associated with them as well.
- the cell structure can be complex, and difficult to produce. Greater complexity often leads to higher manufacturing costs.
- some of the non-oxide types of tandem cells can be susceptible to photo-induced corrosion. (Photo-oxidation usually occurs on the oxygen-generating side of the cell, where non-oxide surfaces tend to become oxidized, instead of liberating oxygen. According to the overall oxidation-reduction scheme, if the oxide layer becomes thick enough, then the photo-induced generation of hydrogen will diminish, effectively shutting down the cell).
- the devices should be capable of producing hydrogen efficiently and economically. Novel photocatalysts used in such devices would also be of great interest.
- the photocatalysts would be capable of functioning as one or more semiconductor electrodes for the device, and should be obtainable and usable at reasonable cost. More specifically, the photocatalysts should exhibit bandgap characteristics which permit very effective absorption of solar radiation and conversion to hydrogen.
- One embodiment of this invention is directed to a photoelectrolysis cell, comprising:
- Ln is at least one lanthanide element
- M is an alkaline earth metal selected from the group consisting of calcium, strontium, barium, and combinations thereof;
- Another embodiment is directed to a method for producing hydrogen in a photoelectrolysis cell which comprises a photoelectrode and a counter-electrode, each electrode being in contact with an electrolyte; wherein the electrodes are also connected (directly or indirectly) through an electrical circuit capable of carrying an electrical load.
- the method comprising the following steps:
- the photoelectrode comprises a material having the formula (Ln 1 ⁇ x M x )(Nb 1 ⁇ y Ta y )O 1+x N 2 ⁇ x , as set forth above.
- Still another embodiment is directed to the photoelectrode itself, formed of the material described herein.
- the photoelectrode is useful for a variety of electrochemical reactions. Various features and advantages for these embodiments will become apparent from a review of the following specification.
- FIG. 1 is a schematic cross-section depicting a photoelectrolysis device according to some embodiments of the invention.
- the photoelectrolysis cell of the present invention can assume a number of structural configurations. Photoelectrolytic cells are described in many references. Non-limiting examples include U.S. Pat. No. 4,090,933 (Nozik) and U.S. Pat. No. 4,172,925 (Chen et al), which are both incorporated herein by reference.
- the photoelectrolysis cell includes a photoelectrode and a counter-electrode, which can be connected to each other in various ways. For example, each electrode could be partially or fully immersed in a liquid electrolyte, and spaced from the other. The electrodes could also be incorporated into a conventional electrical circuit with suitable conductors, as depicted in FIG. 1 (discussed below).
- the photoelectrode and the counter-electrode could be physically attached to each other, e.g., without the need for wire connections between them.
- the photoelectrode e.g., a photoanode
- the counter-electrode e.g., a photocathode
- the photoelectrode comprises a material having the formula (Ln 1 ⁇ x M x )(Nb 1 ⁇ y Ta y )O 1+x N 2 ⁇ x (I)
- Ln is at least one lanthanide element
- x and y are values within the ranges described above. (Each “x” value is taken individually, e.g., it can differ in quantity from the other).
- the lanthanide can be any of the rare earth elements, i.e., lanthanum, cerium, praseodymium, neodymium, promethium, samarium, europium, gadolinium, terbium, dysprosium, holmium, erbium, thulium, ytterbium, and lutetium. Mixtures of two or more of the lanthanides are also possible.
- yttrium and scandium are also considered to be a part of the lanthanide family. (Those skilled in the art understand that yttrium and scandium are chemically similar to members of the rare earth group).
- a specific group of lanthanides for some embodiments comprises at least one of lanthanum, yttrium, gadolinium, lutetium, scandium, neodymium, and praseodymium.
- the lanthanide is selected from the group consisting of lanthanum, lutetium, yttrium, and various combinations thereof.
- M is an alkaline earth metal, selected from the group consisting of calcium, strontium, barium, and combinations thereof. These alkaline earth metals are optional, and can be used in some cases to control the band gap value in the host lattice of the compound. In some specific embodiments, calcium and strontium are the preferred alkaline earth metals, with calcium often being most preferred.
- the photoelectrode material also includes at least one transition metal selected from tantalum and niobium. Tantalum is the preferred transition metal for most embodiments. Combinations of tantalum and niobium are also possible.
- the presence of the oxynitride species in formula (I) provides a degree of photostability to the compound.
- Nirogen is less electronegative than oxygen, and oxynitride compounds have a much lower tendency to oxidize than pure nitride compounds.
- some portion of oxygen may be incorporated into the lattice structure of the compound.
- the oxygen may form oxides, e.g., various lanthanide-tantalum-oxide compounds. These oxides can function as a thin, protective layer for the photoelectrode.
- oxides e.g., various lanthanide-tantalum-oxide compounds.
- the photoelectrode e.g., the anodic electrode
- E g bandgap energy value
- Compounds with this bandgap characteristic are thought to be more efficient in the photoelectrochemical splitting of water, and can thereby utilize a greater portion of the solar spectrum for hydrogen production.
- the photoelectrode will have a bandgap energy in the range of about 1.5 to about 2.0.
- Non-limiting examples of specific compounds for the photoelectrode are as follows: LaTaON 2 ; LuTaON 2 ; LaNbON 2 ; La 0.5 Ca 0.5 TaO 1.5 N 1.5 ; GdTaON 2 ; NdTaON 2 ; YTaON 2 ; GdNbON 2 ; NdNbON 2 ; and various combinations thereof.
- the photoelectrode comprises LaTaON 2 .
- Choice of a particular compound will depend on various factors. They include: the specific type of photoelectrochemical cell (e.g., the type of electrode and counter-electrode employed); the amount of hydrogen production required from the cell; various processing considerations; and material costs.
- a lanthanide oxide can be dry-mixed with tantalum oxide and/or niobium oxide, and then heated in a suitable reactor, under the flow of a nitrogen-containing gas like ammonia.
- a nitrogen-containing gas like ammonia.
- the counter-electrode for the photoelectrolysis cell can be formed from a variety of conventional metallic materials, e.g., pure metals, metal oxides, or metal alloys. Some of them are described in U.S. Pat. No. 4,466,869 (Ayers), which is incorporated herein by reference, as well as in other references which relate to various photolytic processes.
- suitable counter-electrode materials include Group VIII metals, such as iron, cobalt, nickel, rhodium, ruthenium, palladium, osmium, iridium, platinum, and various combinations thereof.
- the counter-electrode material comprises nickel, platinum, palladium, or combinations thereof. Choice of a particular material for the counter-electrode will depend in part on many of the parameters set forth above for the photocathode.
- the photoelectrode for the electrolysis cell is an anodic electrode comprising an n-type material.
- photo-oxidation occurs at the photoelectrode, and oxygen is formed.
- the photoelectrode material described herein could alternatively be used to form a cathodic, p-type electrode material.
- the principles of operation for the photoelectrolysis cell would generally remain the same, although electrical current would flow in the opposite direction, as compared to the depiction of FIG. 1 (further described below).
- photo-reduction occurs at the photoelectrode, where hydrogen is formed.
- the counter-electrode would function as the anode, i.e., the site where photo-oxidation is occurring, and oxygen is formed.
- the electrolyte is a liquid, and can be acidic, basic, or neutral.
- the electrolyte often comprises an aqueous solution, or some other type of polar solvent, such as methanol, ethanol, and the like.
- the electrolyte is basic, and includes a compound such as sodium hydroxide, potassium hydroxide calcium hydroxide, sodium sulfate; or combinations comprising any of the foregoing, to provide a solution having a pH greater than about 7.
- the electrolyte can include other conventional constituents as well.
- the electrolyte composition is one which is substantially non-reactive with either the photoelectrode or the counter-electrode, so that unwanted side reactions can be prevented. It is also usually preferable that the electrolyte be free of constituents which would significantly “plate out” onto the electrodes during operation of the cell.
- FIG. 1 is a schematic cross-section which depicts the structure of a photoelectrolysis device according to one embodiment of the present invention.
- Cell 10 includes photoelectrode 12 (here, the anode), and counter-electrode 14 (here functioning as the cathode). Each electrode is immersed in electrolyte 16 , which itself is contained in any conventional vessel 18 .
- Photoelectrode 12 is capable of absorbing visible light (“hv”) in the desired bandgap values set forth previously.
- counter-electrode 14 is transparent, and also capable of absorbing visible light.
- Conductors 20 and 22 provide connection for the photoelectrode and counter-electrode to a conventional electrical load 24 .
- a switch (not shown) may also be incorporated into the electrical circuit.
- reactions (I) and (II) occur simultaneously in an aqueous electrolyte.
- the incoming light (radiation) is usually described in terms of “hv” (see FIG. 1 ), wherein “h” is Planck's constant (6.62 ⁇ 10 ⁇ 27 erg sec), and “v” is the frequency of radiation in sec ⁇ 1 .
- the incoming radiation hv must be equal or greater than the bandgap energy E g , in order to generate the electron-hole pairs.
- the use of the specific photoelectrodes described previously surpasses these bandgap energy requirements, so that the conversion efficiency of solar radiation can be increased considerably.
- photoelectrolysis cell 10 design of photoelectrolysis cell 10 are possible.
- the alternative designs are described in a variety of references, including some of the patents mentioned in this disclosure. It is expected that the use of the photoelectrodes described herein will provide notable improvements in various aspects of these other types of cells.
- each type of photoelectrolysis cell described in the literature may include a variety of features not specifically set forth herein. Thus, photoelectrolysis cells which include such features are also considered to be part of the scope of this invention.
- the collection and storage of hydrogen gas produced by photoelectrolysis cell 10 is readily accomplished by conventional techniques, e.g., see U.S. Pat. No. 4,090,933, referenced above.
- pressurizable tanks could be used to store the gas which typically bubbles up through the electrolyte as it is produced. (Frequently, the gas is dried and compressed after being generated in the cell).
- the hydrogen can be absorbed by various metals, e.g., to form reversibly-decomposable metal hydrides or other compounds. Those skilled in the art will be able to determine the most appropriate storage system for a given situation. Methods for collecting and storing other gasses produced in the cell, such as oxygen, are also known in the art.
- the photoelectrolysis cell described herein can be used to carry out various important objectives.
- the cell can produce both hydrogen and oxygen. Both gases are very useful for a variety of applications.
- the cell can efficiently convert solar radiation to electrical energy.
- the hydrogen produced by the photoelectrolysis cell can be used in any application requiring the gas.
- Non-limiting examples include fuel cells; internal combustion engines; turbines or other types of engines which rely on hydrogen fuel; and chemical processes which require hydrogen, e.g., hydrogenation systems.
- Those skilled in the art are familiar with the design of systems and processes which employ hydrogen gas.
Abstract
Description
-
- (a) a photoelectrode, comprising
(Ln1−xMx)(Nb1−yTay)O1+xN2−x.
- (a) a photoelectrode, comprising
-
- (b) a counter-electrode comprising at least one metallic material;
- (c) an electrolyte in contact with both the photoelectrode and the counter-electrode; and
- (d) means for collecting hydrogen produced by the cell.
(Ln1−xMx)(Nb1−yTay)O1+xN2−x (I)
In formula (I), Ln is at least one lanthanide element; and x and y are values within the ranges described above. (Each “x” value is taken individually, e.g., it can differ in quantity from the other). In some embodiments, the lanthanide can be any of the rare earth elements, i.e., lanthanum, cerium, praseodymium, neodymium, promethium, samarium, europium, gadolinium, terbium, dysprosium, holmium, erbium, thulium, ytterbium, and lutetium. Mixtures of two or more of the lanthanides are also possible. For the purpose of this disclosure, yttrium and scandium are also considered to be a part of the lanthanide family. (Those skilled in the art understand that yttrium and scandium are chemically similar to members of the rare earth group).
H2O+2h+→2H++½(O2) (I).
The primary reaction which occurs at the counter-electrode (cathode) generates hydrogen:
2H++2e−→H2 (II),
wherein holes are designated as “h+” and electrons are designated as “e−”. As those skilled in the art understand (e.g., see the Nozik patent), reactions (I) and (II) occur simultaneously in an aqueous electrolyte. The incoming light (radiation) is usually described in terms of “hv” (see
Claims (25)
(Ln1−xMx)(Nb1−yTay)O1+xN2−x;
(Ln1−xMx)(Nb1−yTay)O1+xN2−x
(Ln1−xMx)(Nb1−yTay)O1+xN2−x
(Ln1−xMx)(Nb1−yTay)O1+xN2−x
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US11/394,881 US7481914B2 (en) | 2006-03-31 | 2006-03-31 | Photoelectrolysis cells, and related devices and processes |
JP2007080893A JP5306606B2 (en) | 2006-03-31 | 2007-03-27 | Photoelectrolyzer and related apparatus and method |
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Cited By (1)
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US20120237842A1 (en) * | 2010-12-28 | 2012-09-20 | Panasonic Corporation | Optical semiconductor and method for producing the same, optical semiconductor device, photocatalyst, hydrogen producing device, and energy system |
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EP2350347A1 (en) * | 2008-10-08 | 2011-08-03 | Massachusetts Institute of Technology | Catalytic materials, photoanodes, and photoelectrochemical cells for water electrolysis and other electrochemical techniques |
JP4494528B1 (en) * | 2008-10-30 | 2010-06-30 | パナソニック株式会社 | Photoelectrochemical cell and energy system using the same |
JP5493449B2 (en) * | 2009-04-22 | 2014-05-14 | パナソニック株式会社 | Photocatalytic hydrogen generation device |
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JP2011105534A (en) * | 2009-11-15 | 2011-06-02 | Haruo Ota | Hydrogen supply apparatus for internal combustion engine and fuel cell |
WO2011140561A1 (en) * | 2010-05-07 | 2011-11-10 | Molycorp Minerals Llc | Lanthanide-mediated photochemical water splitting process for hydrogen and oxygen generation |
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US20140305805A1 (en) | 2013-04-12 | 2014-10-16 | Uchicago Argonne, Llc | Subnanometer catalytic clusters for water splitting, method for splitting water using subnanometer catalyst clusters |
US20150114832A1 (en) * | 2013-10-24 | 2015-04-30 | Gary Nicholson | Electrochemical device for producing hydrogen |
DE102014107268A1 (en) * | 2014-05-22 | 2015-11-26 | H1 Energy Bv | Energy conversion system |
CN107541747B (en) * | 2016-06-27 | 2019-02-19 | 中国科学院金属研究所 | A kind of energy storage device integrating optical electro-chemical water decomposes the design method of battery |
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US20120237842A1 (en) * | 2010-12-28 | 2012-09-20 | Panasonic Corporation | Optical semiconductor and method for producing the same, optical semiconductor device, photocatalyst, hydrogen producing device, and energy system |
US8663435B2 (en) * | 2010-12-28 | 2014-03-04 | Panasonic Corporation | Optical semiconductor and method for producing the same, optical semiconductor device, photocatalyst, hydrogen producing device, and energy system |
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US20070227896A1 (en) | 2007-10-04 |
JP2007297268A (en) | 2007-11-15 |
JP5306606B2 (en) | 2013-10-02 |
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